Effect of PEG Architecture on the Hybridization Thermodynamics and Protein Accessibility of PEGylated Oligonucleotides

Jia, Fei; Lu, Xueguang; Tan, Xuyu; Wang, Dali; Cao, Xueyan; Zhang, Ke

doi:10.1002/anie.201610753

Cited by 45 publications

(51 citation statements)

References 43 publications

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“…The dramatic increase of the T m of the PEGylated DNA duplexes is indicative of higher thermal stability due to electrostatic PEGylation. The increase in the thermostability could be an effect of intrinsic crowding associated with the PEGylated strands, 66 alteration in the base-pairing kinetics, 67 the overall brush-type architecture of the PEGylated DNA molecules 68 or a combination of them. Other factors, that might play a substantial role in increasing the melting temperature of PEG-coated dsDNA include the excluded volume effect of PEG that can increase the effective concentration of the oligonucleotide leading to more favorable binding, osmotic pressure, DNA condensation or change in dielectric property of the reaction medium.…”

Section: Stability Of Pegylated Dnamentioning

confidence: 99%

Electrostatically PEGylated DNA enables salt-free hybridization in water

et al. 2019

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Section: Stability Of Pegylated Dnamentioning

confidence: 99%

Electrostatically PEGylated DNA enables salt-free hybridization in water

et al. 2019

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“…Such DNAa ptamers not only exhibit specific and high affinity toward cancer cells by enhanced receptor-mediated internalization but also serve to functionalize the HBP as the hydrophilic shell to enable HBP-DNAnanoparticle (HDNP) self-assembly and enhance colloidal stability of this amphiphilic nanostructure. [10] Forthe UV-responsive hydrophobic core of the delivery system, aH BP-containing pendent o-nitrobenzyl moieties was synthesized. Moreover,api-pi stacking effect arising from nitrobenzyl rings is also believed to contribute to selfassembly.P hotoredox chemistry of o-nitrobenzyl derivatives will occur after UV irradiation, resulting in the liberation of free carboxylic acid groups and enhanced hydrophilicity of the core.…”

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confidence: 99%

Self‐Assembled Aptamer‐Grafted Hyperbranched Polymer Nanocarrier for Targeted and Photoresponsive Drug Delivery

et al. 2018

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Photoresponsive materials are emerging as ideal carriers for precise controlled drug delivery owing to their high spatiotemporal selectivity. However, drawbacks such as slow release kinetics, inherent toxicity, and lack of targeting ability hinder their translation into clinical use. We herein constructed a new DNA aptamer-grafted photoresponsive hyperbranched polymer, which can self-assemble into nanoparticles, thereby achieving biocompatibility and target specificity, as well as light-controllable release behavior. Upon UV-irradiation, rapid release induced by disassembly was observed for Nile Red-loaded nanoparticles. Further in vitro cell studies confirmed this delivery system’s specific binding and internalization performance arising from the DNA aptamer corona. The DOX-loaded nanoassembly exhibited selective phototriggered cytotoxicity towards cancer cells, indicating its promising therapeutic effect as a “smart” drug delivery system.

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“…33,34 Yet, excluded volume also restricts the degrees of freedom of hybridizing molecules and biases the DNA toward more enthalpically stable conformations. This effect is reminiscent of the stability observed for locked nucleic acid (LNA) hybridization.…”

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confidence: 99%

The Role of Structural Enthalpy in Spherical Nucleic Acid Hybridization

Fong¹,

Wang²,

Schatz³

et al. 2018

J. Am. Chem. Soc.

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DNA hybridization onto DNA-functionalized nanoparticle surfaces (e.g., in the form of a spherical nucleic acid (SNA)) is known to be enhanced relative to hybridization free in solution. Surprisingly, via isothermal titration calorimetry, we reveal that this enhancement is enthalpically, as opposed to entropically, dominated by ~20 kcal/mol. Coarse-grained molecular dynamics simulations suggest that the observed enthalpic enhancement results from structurally confining the DNA on the nanoparticle surface and preventing it from adopting enthalpically unfavorable conformations like those observed in the solution case. The idea that structural confinement leads to the formation of energetically more stable duplexes is evaluated by decreasing the degree of confinement a duplex experiences on the nanoparticle surface. Both experiment and simulation confirm that when the surface-bound duplex is less confined, i.e., at lower DNA surface density or at greater distance from the nanoparticle surface, its enthalpy of formation approaches the less favorable enthalpy of duplex formation for the linear strand in solution. This work provides insight into one of the most important and enabling properties of SNAs and will inform the design of materials that rely on the thermodynamics of hybridization onto DNA-functionalized surfaces, including diagnostic probes and therapeutic agents.

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Effect of PEG Architecture on the Hybridization Thermodynamics and Protein Accessibility of PEGylated Oligonucleotides

Cited by 45 publications

References 43 publications

Electrostatically PEGylated DNA enables salt-free hybridization in water

Electrostatically PEGylated DNA enables salt-free hybridization in water

Self‐Assembled Aptamer‐Grafted Hyperbranched Polymer Nanocarrier for Targeted and Photoresponsive Drug Delivery

The Role of Structural Enthalpy in Spherical Nucleic Acid Hybridization

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